Electrocatalytic CO2 reduction to CO is a sustainable process for energy conversion.However,this process is still hindered by the diffusi limited mass transfer,low electrical conductivity and catalytic activity.Theref...Electrocatalytic CO2 reduction to CO is a sustainable process for energy conversion.However,this process is still hindered by the diffusi limited mass transfer,low electrical conductivity and catalytic activity.Therefore,new strategies for catalyst design should be adopted to solve these problems and improve the electrocatalytic performa nee for CO production.Herein,we report a multiscale carb on foam confining〔single iron atoms prepared with the assistant of S1O2 template.The pore-enriched environment at the macro-scale facilitates the diffusion of reacta nts and products.The graphe ne nano sheets at the nano-scale promote the charge tran sfer duri ng the reaction.The single iron atoms con fined in carb on matrix at the atomic-scale provide the active sites for electrocatalytic CO2 reductio n to CO.The optimized catalyst achieves a CO Faradaic efficiency of 94.9%at a moderate potential of-0.5 V vs.RHE.Furthermore,the performance can be maintained over 60 hours due to the stable single iron atoms coordi nated with four n itroge n atoms in the carb on matrix.This work provides a promising strategy to improve both the activity and stability of single atom catalysts for electrocatalytic CO2 reduction to CO.展开更多
基金We gratefully acknowledge the financial support from the Ministry of Science and Technology of China(Nos.2016YFA0204100 and 2016YFA0200200)the National Natural Science Foundation of China(Nos.21573220 and 21802124)+2 种基金the Key Research Program of Frontier Sciences of the Chinese Academy of Sciences(No.QYZDB-SSW-JSC020)the DNL Cooperation Fund,CAS(No.DNL180201)We thank staff at the BL14W1 beamline of the Shanghai Synchrotron Radiation Facilities(SSRF)for assistance with the X-ray absorption spectroscopy measurements.
文摘Electrocatalytic CO2 reduction to CO is a sustainable process for energy conversion.However,this process is still hindered by the diffusi limited mass transfer,low electrical conductivity and catalytic activity.Therefore,new strategies for catalyst design should be adopted to solve these problems and improve the electrocatalytic performa nee for CO production.Herein,we report a multiscale carb on foam confining〔single iron atoms prepared with the assistant of S1O2 template.The pore-enriched environment at the macro-scale facilitates the diffusion of reacta nts and products.The graphe ne nano sheets at the nano-scale promote the charge tran sfer duri ng the reaction.The single iron atoms con fined in carb on matrix at the atomic-scale provide the active sites for electrocatalytic CO2 reductio n to CO.The optimized catalyst achieves a CO Faradaic efficiency of 94.9%at a moderate potential of-0.5 V vs.RHE.Furthermore,the performance can be maintained over 60 hours due to the stable single iron atoms coordi nated with four n itroge n atoms in the carb on matrix.This work provides a promising strategy to improve both the activity and stability of single atom catalysts for electrocatalytic CO2 reduction to CO.